(001)-oriented heterostructures consisting of LaAlCO3 substrates, SrRuO3 bottom electrodes, and Pb(Mg1/3Nb2/3) O3-PbTiO3 (PMN-PT) piezoelectric actuators were deposited by pulsed laser deposition (PLD). 4-circle x-ray diffraction analysis confirmed the epitaxial growth of each layer. In general, the electrical properties were found to be very sensitive to the processing conditions, in particular, the growth temperature. At growth temperatures below ∼620°C, the temperature dependence of the dielectric constant and the onset of a hysteritic polarization were found to be depressed by as much as 80 °C. When growth temperatures were increased above 660°C, electrical properties with temperature dependencies more consistent with those of single crystals were observed.